Supramolecular systems feature dynamic, reversible and stimuli-responsive characteristics, which are not easily achieved by molecular entities. The last decade has witnessed tremendous advances in the investigations of supramolecular systems for various bioapplications, which include drug delivery, anticancer therapy, antibacterial therapy, photodynamic therapy, photothermal therapy, combination therapy, antidotes for residual drugs or toxins, and bioimaging and biosensing. Host-guest chemistry has played a key role in the development of such bioactive supramolecular systems, and natural macrocycles (such as cyclodextrins), synthetic macrocycles (such as calixarenes, cucurbit[n]urils, and pillararenes), and porous framework polymers (such as supramolecular organic frameworks and flexible organic frameworks) have been most successfully used as hosts to build different kinds of host-guest systems for attaining designed biofunctions. The self-assembly of rationally designed amphiphilic molecules, macromolecules and polymers represent another important approach for the construction of supramolecular architectures with advanced biofunctions. In this review, we summarize the important contributions made by Chinese researchers in this field, with emphasis on those reported in the past five years. (Figure presented.)